Publication Date

12-2017

Department

Ames Laboratory; Materials Science & Engineering; Chemistry

Campus Units

Chemistry, Ames Laboratory

Report Number

IS-J 9489

DOI

10.1016/j.jcat.2017.10.011

Journal Title

Journal of Catalysis

Volume Number

356

First Page

307

Last Page

314

Abstract

Bridging the structure-properties relationship of bimetallic catalysts is essential for the rational design of heterogeneous catalysts. Different from random alloys, intermetallic compounds (IMCs) present atomically-ordered structures, which is advantageous for catalytic mechanism studies. We used Pt-based intermetallic nanoparticles (iNPs), individually encapsulated in mesoporous silica shells, as catalysts for the hydrogenation of nitroarenes to functionalized anilines. With the capping-free nature and ordered atomic structure, PtSn iNPs show >99% selectivity to hydrogenate the nitro group of 3-nitrostyrene albeit with a lower activity, in contrast to Pt3Sn iNPs and Pt NPs. The geometric structure of PtSn iNPs in eliminating Pt threefold sites hampers the adsorption/dissociation of molecular H2 and leads to a non-Horiuti-Polanyi hydrogenation pathway, while Pt3Sn and Pt surfaces are saturated by atomic H. Calculations using density functional theory (DFT) suggest a preferential adsorption of the nitro group on the intermetallic PtSn surface contributing to its high selectivity.

Language

en

Department of Energy Subject Categories

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Publisher

Iowa State University Digital Repository, Ames IA (United States)

IS-J 9489 SI.pdf (832 kB)
Supplementary Information

Available for download on Tuesday, November 27, 2018

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